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Metal Ion Collection Systems Based on the Ligned Basicity Change on Redox Reactions of Some Metal Complexes

Research Project

Project/Area Number 09554037
Research Category

Grant-in-Aid for Scientific Research (B).

Allocation TypeSingle-year Grants
Section展開研究
Research Field Inorganic chemistry
Research InstitutionHOKKAIDO UNIVERSITY

Principal Investigator

SASAKI Yoichi  Hokkaido Univ., Grad.School of Sci., Prof., 大学院・理学研究科, 教授 (30004500)

Co-Investigator(Kenkyū-buntansha) KANESATO Masatoshi  Tohoku National Industrial Research Institute, Functional Molecules Section, Senior Researcher, 東北工業技術研究所・機能化学部, 主任研究官
SUZUKI Toshishige  Tohoku National Industrial Research Institute, Chief Senior Researcher, 東北工業技術研究所, 首席研究官
ABE Masaaki  Hokkaido Univ., Grad.school of Sci., Inst., 大学院・理学研究科, 助手 (90260033)
Project Period (FY) 1997 – 2000
Project Status Completed (Fiscal Year 2000)
Budget Amount *help
¥11,100,000 (Direct Cost: ¥11,100,000)
Fiscal Year 2000: ¥2,800,000 (Direct Cost: ¥2,800,000)
Fiscal Year 1999: ¥2,500,000 (Direct Cost: ¥2,500,000)
Fiscal Year 1998: ¥2,200,000 (Direct Cost: ¥2,200,000)
Fiscal Year 1997: ¥3,600,000 (Direct Cost: ¥3,600,000)
KeywordsMetal-Metal Bond / Transition Metal Elements / Functional Electrode / Enzyme Model Complexes / Metal Cluster Complexes / Redox Reactions / Electrode Reactions / Catalytic Reactions
Research Abstract

Basicity of oxide bridge of dinuclear complexes changes remarkably with the change in the oxidation states of the metal ions. It is thus possible to control the interaction of the oxide bridge with various Lewis acids like metal ions by changing the metal oxidation states. This work aimed at preparing the electrodes with surface self-assembled monolayers of such metal complexes, and use them as reversible metal-ion binder and to establish the method for the step-wise construction of metal-complex oligomers. The results are summarized as follows.
(1)Methods to construct Au self-assembled monolayers of polynuclear metal complexes have been established by using(i)mixed monolayers with alkyl sulfide and(ii)hydrogen bonding between the chains which contain C-CO-NH-groups.
(2)Protoncoupled electron transfer behavior of the oxo-bridged biruthenium complexes on gold surface have been quantitatively investigated. Diiron alnalaogs which are considered as models of biological diiron centers and are unstable towards redox reactions in solution, have been successfully studied in terms of pH-potential profiles over pH range of 1 and 12. The pKa values of the oxidized and reduced forms have been estimated for the first time for the model Fe-O-Fe complexes.
(3)Coupled redox reactions have been studied quantitatively with Lewis acids other than proton for the first time. Thus, for example, interaction of Al^<3+> ions at the oxide bridge is more sensitive to the metal ion oxidation states than protons.
(4)Step-wise oligomerization of the trinuclear oxo-centered Ru complexes on Au electrode has been established by controlling the metal oxidation state. The method is promising in contructing various supramolecular assemblies on electrode surfaces.

Report

(5 results)
  • 2000 Annual Research Report   Final Research Report Summary
  • 1999 Annual Research Report
  • 1998 Annual Research Report
  • 1997 Annual Research Report
  • Research Products

    (36 results)

All Other

All Publications (36 results)

  • [Publications] Hiroshi Kumagai: "Chromatographic Selectivity of Rare Earth Elements on Iminodiacetate-Type Chelating Resins Having Spacer Arms of Different Lengths : Importance of Steric Flexibility of Functional Group in a Polymer Chelating Resin."Analytical Chmeistry. 70(No.1). 19-24 (1998)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] Masaaki Abe: "Synthesis and Electochemical Characterization of Self-Assembled Monolayers of Redox-Active Oxide-Bridged Triruthenium (III) Clusters on Au (111)."Journal of the Electroanalytical Chemistry. 473(No.1-2). 93-98 (1999)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] Pu Quan: "Chiral Molecular Patterns of Self-assembled Ion Pairs Composed of (R,S), (S)-16-Methyloctadecanoic Acid and 4,4'-Bipyridine."Chemical Communications. No.22. 2021-2022 (2000)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] Masaaki Abe: "Characterization of Novel Redox-Active Triruthenium (III) Complexes with a Disulfide-alkyl Ligand. Anion-Dependent Redox Behaviour of Monolayer Assemblies on Gold."Journal of the Chemical Society, Dalton Transactions. No.16. 2693-2701 (2000)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] Zhong-Ning Chen: "Chelate Formation around the Hexarhenium Cluster Center by a Diphosphane Ligand, Ph_2P(CH_2)_6PPh_2."Angewandte Chemie, International Edition in English. 40(No.1). 239-242 (2001)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] Akira Sato: "Cyclic Voltammetric Observation of CO/aqua Terminal Ligand Substitution Reactions for Trinuclear Ruthenium Complexes at Self-Assembled Monolayer Interfaces."Physical Chemistry Chemical Physics. (印刷中). (2001)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] Hiroshi Kumagai, et al.: "Chromatographic Selectivity of Rare Earth Elements on Iminodiacetate-Type Chelating Resins Having Spacer Arms of Different Lengths : Importance of Steric Flexibiliy of Functional Group in a Polymer Chelating Resin."Analytical Chmeistry. 70(No.1). 19-24 (1998)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] Masaaki Abe, et al.: "Synthesis and Electochemical Characterization of Self-Assembled Monolayers of Redox-Active Oxide-Bridged Triruthenium(III)Clusters on Au(111)."Journal of the Electroanalytical Chemistry. 473(No.1-2). 93-98 (1999)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] Pu Quan, et al.: "Chiral Molecular Patterns of Self-assembled Ion Pairs Composed of (R, S), (S)-16-Methyloctadecanoic Acid and 4, 4'-Bipyridine."Chemical Communications. No.22. 2021-2022 (2000)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] Masaaki Abe, et al.: "Characterization of Novel Redox-Active Triruthenium(III)Complexes with a Disulfide-alky Ligand. Anion-dependent Redox Behavior of Monolayer Assemblies on Gold."Journal of the Chemical Society, Dalton Transactions. No.16. 2693-2701 (2000)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] Zhong-Ning Chen, et al.: "Chelate Formation around the Hexarhenium Cluster Center by a Diphosphane Ligand, Ph_2P(CH_2)_6PPh_2."Angewandte Chemie, International Edition in English. 40(No.1). 239-242 (2001)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] Akira Sato, et al.: "Cyclic Voltammetric Observation of CO/aqua Terminal Ligand Substitution Reactions for Trinuclear Ruthenium Complexes at Self-Assembled Monolayer Interfaces."Physical Chemistry Chemical Physics. (in press). (2001)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2000 Final Research Report Summary
  • [Publications] Zhong-Ning Chen: "Chelate Formation around the Hexarhenium Cluster Center by a Diphosphane Ligand, Ph_2P (CH_2)_6PPh_2."Angewandte Chemie. International Edition in English. 40(No.1). 239-242 (2001)

    • Related Report
      2000 Annual Research Report
  • [Publications] Toshishige M.Suzuki: "Adsorption and Removal of Oxo-Anions of Arsenic and Selenium on the Zirconium (IV) Loaded Polymer Resin Functionalized with Diethelenetriamine-N, N, N'N'-polyacetic Acid."Journal of Environmental Monitoring. 2(No.2). 550-555 (2000)

    • Related Report
      2000 Annual Research Report
  • [Publications] Pu Qian: "Self-Assembly of Alkyl Substituted Schiff Base and Its Cu) II) Complex Observed on Solution-Graphite Interface by Scanning Tunneling Microscopy"Chemistry Letters. No.11. 1118-1119 (2000)

    • Related Report
      2000 Annual Research Report
  • [Publications] Akira Sato: "Cyclic Voltammetric Observation of CO/aqua Terminal Ligand Substitution Reactions for Trinuclear Ruthenium Complexes at Self-Assembled Monolayer Interfaces."Physical Chemistry Chemical Physics. (印刷中). (2001)

    • Related Report
      2000 Annual Research Report
  • [Publications] Masaaki Abe: "Characterization of Novel Redox-Active Triruthenium (III) Complexes with a Disulfide-alkyl Ligand. Anion-Dependent Redox Behaviour of Monolayer Assemblies on Gold."Journal of the Chemical Society, Dalton Transactions. No.16. 2693-2701 (2000)

    • Related Report
      2000 Annual Research Report
  • [Publications] J.Folorunso Ojo: "Kinetics of the Reduction of Tris (1,10-phenanthroline) iron (III) and Emission Quenching of Tris (2, 2'-bipyridine) ruthenium (II) by Di-and Tri-nuclear Oxo-Acetato Bridged Ruthenium Complexes. Inorg. React. Mech., in press (2001)."Inorganic Reaction Mechanisms. 4巻(印刷中). (2001)

    • Related Report
      2000 Annual Research Report
  • [Publications] Keisuke Umakoshi: "Synthesis and Redox Properties of Amino Acid-Bridged Dinuclear Iron (III) Complexes"Bull. Chem. Soc. Jpn.. 72(3). 433-440 (1999)

    • Related Report
      1999 Annual Research Report
  • [Publications] Tomohiko Inomata: "Interaction of Some Lewis Acids with the Oxo-bridge of (μ-Oxo)di(μ-acetato)diruthenium (III,III) Complexes and Their Electrochemical Consequence"Electrochem.. 67(5). 427-430 (1999)

    • Related Report
      1999 Annual Research Report
  • [Publications] Masaaki Abe: "Enhanced Kinetic Lability of Ru(III) Centers in Oxo-Centered Mixed-Metal Ru_2M Trinuclear Complexes (M=Zn and Mg)"Inorg. Chem.. 38(18). 4146-4148 (1999)

    • Related Report
      1999 Annual Research Report
  • [Publications] Masaaki Abe: "Synthesis and Electrochemical Characterization of Self-Assembled Monolayers of Redox-Active Oxide-Bridged Triruthenium(III) Clusters on Au(III)"J. Electroanal. Chem.. 473(1-2). 93-98 (1999)

    • Related Report
      1999 Annual Research Report
  • [Publications] Tomohiko Inomata: "Self-Assembled Monolayers of Non-Heme Diiron(III) Model Complexes on Au(111) Electrode : Synthesis and Proton-Coupled Redox Behavior in Water"Chem. Lett.. No.10. 1097-1098 (1999)

    • Related Report
      1999 Annual Research Report
  • [Publications] Masaaki Abe: "Electrochemical and Infrared Spectroelectrochemical Characterization of Self-Assembled Monolayers of a Carbonyl-Coordinated Trinuclear Ruthenium Complex on a Gold Electrode"Electrochem.. 67(12). 1162-1164 (1999)

    • Related Report
      1999 Annual Research Report
  • [Publications] H.Sugimoto: "Oxorhenium(V)Complex of Amidophenolate: Structure and Redox Characteristics." Chem.Lett.3. 197-198 (1998)

    • Related Report
      1998 Annual Research Report
  • [Publications] M.Akiba: "A Platinum(II) Complex Containing Carbon-Bonded ‘Nitromethane': [Pt(CH_2NO_2)(2,2':6,2"-terpyridine)]^+." Inorg.Chem.Comm.1(No.2). 61-63 (1998)

    • Related Report
      1998 Annual Research Report
  • [Publications] J.M.Botha: "Chelation porcesses to an Oxorhenium(V) Center by N,N,N,O-Tetradentate and N,N,O-Tridentate Ligands as Verified by Structural and Mechanistic Studies of Intermediate Species." Inorg.Chem.37(No.7). 1609-1615 (1998)

    • Related Report
      1998 Annual Research Report
  • [Publications] T.Fukumoto: "Preparation and Properties of a Series of the(μ-Oxo)di(μ-acetato)diruthenium(III) Complexes. [Ru_2(μ-O)(μ-CH_3COO)_2(Pyridine)_4(L)_2]^<2+> and [Ru_2(μ-O)(μ-CH_3COO)_2(AA)_2(L)_2]^<2+>, where AA is 2,2'-Bipyridine or 1,10-Phenanthroline, and L is a Monodenatte Ligand." Inorg.Chem.Acta.283(No.1). 151-159 (1998)

    • Related Report
      1998 Annual Research Report
  • [Publications] K.Funatsu: "Novel Cofacial Ruthenium(II) Porphyrin Dimers and Tetramers." Inorg.Chem.37(No.19). 4986-4995 (1998)

    • Related Report
      1998 Annual Research Report
  • [Publications] M.Abe: "Syntheses, Structures and Fluctional Behavior of Tricarbonyl Mo(0) and Trioxo Mo(VI)Complexes of Tris(2-pyridylmethyl)amine with One Free Arm." Chem.Lett.2. 163-164 (1999)

    • Related Report
      1998 Annual Research Report
  • [Publications] Mats Valli: "An in-situ X-ray Absorption Fine Structure Study of Different Oxidation States of Oxo and Hydroxo-Bridged Ruthenium Dimers in Acetonitrile Solution." Inorganic Chemistry. 36(No.21). 4622-4626 (1997)

    • Related Report
      1997 Annual Research Report
  • [Publications] Masaaki Abe: "Lewis Acid Trifluoroboran Coordimation to trans-Dioxorhenium(V)Moiety:Structural and Spectroscopic Characterization of trans-[Re(O)(OBF_3)(1-Meim)_4](BF_4)(Meim=1-methylimidazole)." Chemistry Letters. No.10. 1073-1074 (1997)

    • Related Report
      1997 Annual Research Report
  • [Publications] Toshishige M.Suzuki: "Removal of As(III)and As(V)by a Porous Spherical Resin Loaded with Monoclinic Hydrous Zirconium Oxide" Chemistry Letters. No.11. 1119-1120 (1997)

    • Related Report
      1997 Annual Research Report
  • [Publications] Masaharu Akiba: "A Platinum(II)Complex Containing Carbon-Bonded 'Nitromethane'[Pt(CH_2NO_2)(2,2':6,2"-terpyridine)]^+" Inorganic Chemistry Communications. 1(No.2). 61-63 (1998)

    • Related Report
      1997 Annual Research Report
  • [Publications] Chikako Koshi: "Oxo-Carboxylato Bridged Diruthenium(III)Complexes of Tris(2-pyridylmethyl)amine." Chemistry Letters. No.11. 1155-1156 (1977)

    • Related Report
      1997 Annual Research Report
  • [Publications] Hideki Sugimoto: "Oxorhenium(V)Complex of Amidophenolate:Structure and Redox Characteristics." Chemistry Letters. No.3. 197-198 (1998)

    • Related Report
      1997 Annual Research Report

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Published: 1997-04-01   Modified: 2016-04-21  

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